EDWARDS: Plutonium and Thorium based reactor concepts prior to 1945.
by Dr. Gordon Edwards
April 23, 2011 1:20 AM
HISTORICAL BACKGROUND: THORIUM IN REACTORS
I have received a number of inquiries about "thorium-fueled" nuclear reactors. In order to provide some context, I have decided to circulate some paragraphs that I wrote in 1990-92 under contract to the Canadian Environmental Advisory Council. These excerpts deal with the early history of nuclear research in Montreal during World War II, conducted at a secret laboratory on the slopes of Mount Royal -- a satellite operation connected to the tripartite (US-UK-Canada) Atomic Bomb Project.
Before the end of the war, nuclear scientists had already foreseen the need to go beyond uranium-235 as a nuclear fuel because natural uranium supplies would run out quickly if thousands of "nuclear boilers" were ever built. This motivated a consideration of "advanced fuel cycles" based on either plutonium (a man-made element produced in a reactor when atoms of uranium-238 are bombarded with neutrons) or uranium-233 (a man-made isotope of uranium produced in a reactor when atoms of thorium-232 are bombarded with neutrons). These are very old ideas.
Those not familiar with the early history of the nuclear age are often fooled into thinking that these old ideas are instead very new. Such is the case with the so-called "thorium-fueled" reactors. Thorium is a naturally occurring radioactive material which is approximately three times as abundant as naturally-occurring uranium.
First and foremost, it must be understood that -- unlike uranium -- thorium can NOT be used as a nuclear fuel. If you loaded only thorium "fuel" into a nuclear reactor and "turned the switch", nothing at all would happen. No energy; no heat, no chain reaction; no steam; no electricity; no nothing.
BUT: when thorium is bombarded with neutrons produced by SOME OTHER nuclear fuel, then a fraction of those thorium atoms are transmuted into atoms of uranium-233 -- an isotope of uranium that is not found in nature. Uranium-233, as it happens, is a powerful nuclear explosive material and can also be used to fuel a nuclear reactor. So, although thorium is not a FISSILE material (it cannot be used directly to fuel a reactor or to make atomic bombs) it is a FERTILE material (it "breeds" uranium-233 which can be used either as fuel for a reactor or as an explosive material for bombs.)
In this respect thorium resembles uranium-238, which is also not fissile and not a nuclear explosive material (unlike uranium-235, which is both of those things). Uranium-238 is not fissile, but it is fertile -- because when atoms of uranium-238 absorb a neutron, they are rapidly transmuted into atoms of plutonium-239: a man-made material which is very fissile and also a very powerful nuclear explosive.
So when one hears talk of "thorium reactors" it is important to realize that this only makes sense in the context of an "advanced fuel cycle" that requires the reprocessing of irradiated uranium fuel before anything else can be done.
Reprocessing irradiated uranium fuel entails dissolving the intensely radioactive fuel bundles in boiling nitric acid and then chemically separating the plutonium (typically less than 1 percent) out of the highly radioactive and corrosive witches' brew of liquid wastes that results. Radioactive gases and vapours are released from the irradiated fuel when this is done, and the leftover liquid wastes contain hundreds of heat-generating radioactive materials that were created inside the reactor. The recovered plutonium (a fissile material which can be used as a nuclear fuel or as a nuclear explosive) must then be blended with thorium to produce a "fissile-fertile" hybrid material that can be used to fuel a nuclear reactor, using plutonium as the fuel and thorium as a fertile material that "breeds" uranium-233. That uranium-233 can later be used as a fuel....
In short: ANY discussion of thorium reactors IMPLIES the reprocessing of irradiated nuclear fuel, and the recovery of plutonium from that irradiated fuel, as a first step. Only when that fact is clearly understood can any further useful discussion take place about the different variations that have been advanced by proponents to implement the "thorium cycle" idea.
Gordon Edwards.
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As promised, here is some historical background:
Excerpts from
http://ccnr.org/ceac_C.html
Health and Environmental Issues Linked to the Nuclear Fuel Chain written by Gordon Edwards Ph.D. for the Canadian Environmental Advisory Council
From Section C: Nuclear Fission.
C.20. Canada's First Nuclear Reactor
Finally, on April 13, 1943, in Washington D.C., the Committee decided that a large-scale pilot plant for plutonium production would be built in Canada using heavy water as a moderator. Materials would be provided by the U.S., but no information would be imparted about the chemistry or biomedical hazards of fission products or plutonium. The Montreal team would have to discover all such information for itself using a few irradiated uranium rods donated from U.S. reactors.
The first necessity was to find a firm to design and build the pilot plant in Canada. The natural choice was Defence Industries Limited (DIL), a crown company involved in munitions manufacture, whose key staff was drawn from CIL. On May 18 the DIL Directors were briefed on the nature of a nuclear chain reaction and the basic requirements for a heavy water moderated reactor.
They were told the reactor could not explode like an atomic bomb because it would use only slow neutrons. It was nevertheless clear that an uncontrolled chain reaction would result in a violent release of energy, possibly scattering fission products over a wide area. On several occasions before the first atomic bomb was tested, it had been suggested that great damage might be done to an enemy by dropping fission products from the air, thereby contaminating food and water supplies and making strategic areas uninhabitable. Any similar contamination occurring by accident, it was pointed out, would have a deplorable effect on the future public relations of CIL.
Mackenzie retorted that CIL would surely not escape blame if DIL refused the contract and some less capable firm did the job. That could be seen as evasion of reponsibility. On May 26, DIL accepted the contract, and the search for a site began. For reasons both of safety and security, it would have to be isolated.
The shores of Georgian Bay, Lake Superior and the La Tuque region of Quebec were considered. Finally, in mid-July, a secluded spot on the Ottawa River was selected. It was two hundred miles northwest of the capital, near the small village of Chalk River. A townsite for employees was chosen at Indian Point a few miles away; the community is now known as "Deep River". Deep River was situated far enough upwind and upriver of the Chalk River research reactors to avoid radioactive fallout.
C.21. The Chalk River Nuclear Complex
Meanwhile, the Montreal group had determined the basic features of the Canadian pilot plant, to be called NRX for "National Research Xperiment". The fuel would consist of 175 rods of uranium metal, each with a thin coating of aluminum. The coating, or "cladding", would protect the metallic fuel against chemical reactions and prevent the escape of fission products. The fuel rods would be suspended in an aluminum tank full of heavy water, surrounded by graphite to "reflect" escaping neutrons back into the tank.
Since NRX would generate more than ten million watts of heat, the fuel would have to be cooled to prevent melting. Reliable shutdown systems would be required to halt the chain reaction abruptly if it began to get out of control. Biological shielding would be needed to protect workers from neutrons during operation. In addition, the gamma radiation from fission products would be so intense that massive shielding would be required to safeguard workers at all times, even when the reactor was shut down.
These safety concerns greatly complicated the design of the plant. The NRX fuel rods were to be housed in double-walled tubes through which ordinary "light" water would be pumped at very high speed to cool the fuel. The tubes had to be thin, so as not to absorb too many neutrons, but strong enough to prevent a loss of coolant. The heavy water moderator would fill all the remaining space in the tank outside these vertical tubes. Between the tubes would be hundreds of adjustable "control rods" made of neutron-absorbing materials. When inserted vertically into the tank, these rods would soak up excess neutrons, slowing down or stopping the reaction.
Structural materials near the core of the reactor would inevitably absorb stray neutrons. Due to the resulting activation (see A.21), all of the internal structures, including the cooling tubes and control rods, would become intensely radioactive. Thus, maintenance could be performed only by remote control or after a lengthy shutdown. Given these complications, it was considered prudent to build a much smaller and simpler reactor -- using the same fuel, moderator and reflector as NRX, but not powerful enough to need cooling and not radioactive enough to prevent workers from approaching it. It was to be called ZEEP for "Zero Energy Experimental Pile". [48]
In late July, Cockcroft sent for Lew Kowarski to take charge of the ZEEP project. A member of the original Paris group, Kowarski brought with him some other members of the Cambridge heavy water team who had chosen to stay in England because of personal difficulties with van Halban. The Canadian government had offered to pay the whole shot, but the final cost estimate was something of a shock. It included NRX, ZEEP, two chemical extraction plants, a huge water purification plant and a maze of labs and offices. It also included an entire planned community at Indian Point (the village of Deep River) complete with hospital, school, shopping centre, recreational hall and administration building.
Ottawa gave its approval for the Chalk River complex on August 19, 1944, five days before the liberation of Paris.
C.22. Advanced Reactor Concepts
There were now about 100 scientists in the Montreal group -- over forty Canadians, an equal number of British, and twelve others -- including five French citizens. During the fall of 1944 and the spring of 1945, while detailed design work for NRX and ZEEP was underway, these scientists also found time for other types of advanced research.
The Americans had suggested that in designing the NRX reactor, provision should be made for thorium rods to be inserted in the graphite reflector. By then it was known that thorium-232 changes into fissile uranium-233 by neutron capture, just as uranium-238 changes into fissile plutonium-239. A new man-made isotope of uranium, U-233 could be used as a nuclear explosive and so was worth investigating.
The British were beginning to plan for the post-war period. Having no heavy water in England, they elected graphite as their moderator of choice. A "graphite group" was formed at Montreal in December, 1944, and by the end of the war all the basic design work had been done for Britain's first experimental reactor at Harwell, called BEPO. The graphite for Britain's first few reactors came from Ontario.
Early in 1945 a "future systems group" was formed at Montreal to brainstorm on other possible reactor designs. Special materials able to resist corrosion, conduct heat and tolerate radiation were sought out. A variety of liquids and gases were investigated for possible use as coolants. In the end, this group anticipated every major conceptual development in reactor design for the next quarter century.
In particular, they perceived that economic deposits of uranium are likely to be rather scarce. Accordingly, if nuclear boilers were to last for more than a few decades as an energy source, they saw a need to "breed" a man-made substitute for uranium-235; either plutonium-239 bred from uranium-238, or uranium-233 bred from thorium-232.
They were thus led to conceive a futuristic type of nuclear reactor, fuelled by highly concentrated ("enriched") fissile material, fissioned by fast neutrons rather than slow ones, and surrounded by a blanket of uranium-238 or thorium-232. In principle, more fissile material can be bred in the blanket -- by neutron capture -- than is consumed in the fuel. This greatly extends the supply of nuclear fuel. Such advanced reactors are called "fast breeder reactors", and the stuff in the blanket is appropriately called "fertile material". Experimental breeders have since been built in the U.S., the U.S.S.R. and France.
C.23. Reprocessing Spent Nuclear Fuel
In July, 1944, the U.S. delivered to Canada a few irradiated rods of uranium (containing plutonium), and of thorium (containing U-233). The Montreal chemists knew little about the U.S. method for seperating plutonium except that it was based on precipitation. The Americans would first dissolve the spent fuel in nitric acid, then chemically convert the dissolved plutonium into a solid which would slowly settle out, leaving fission products and uranium in solution.
Precipitation has one big disadvantage: it can only be done in batches. It is a stop-and-start operation. The Montreal team sought a process that would run continuously, producing a steady stream of plutonium. Over two hundred solvents were studied to find one that would strip plutonium away from the other radioactive materials, creating two liquid fractions which, like oil and water, do not mix. The plutonium-bearing fraction could then be separated mechanically and continuously, and from it the plutonium itself could be extracted at will. Similar concepts applied to the separation of U-233.
The British and French both gained a distinct post-war advantage over the U.S. in reprocessing technology -- the technique of recovering fissile material from spent nuclear fuel -- as a result of their Montreal experiences. That advantage persists to the present day.
